Boosting Electrochemical Nitrogen Reduction Performance over Binuclear Mo Atoms on N-Doped Nanoporous Graphene: A Theoretical Investigation

Exploration of efficient catalysts is a priority for the electrochemical nitrogen reduction reaction (NRR) in order to receive a high product yield rate and faradaic efficiency of NH(3), under ambient conditions. In the present contribution, the binding free energy of N(2), NNH, and NH(2) were used as descriptors to screen the potential NRR electrocatalyst among different single or binuclear transition metal atoms on N-doped nanoporous graphene. Results showed that the binuclear Mo catalyst might exhibit the highest catalytic activity. Further free energy profiles confirmed that binuclear Mo catalysts possess the lowest potential determining step (hydrogenation of NH(2)* to NH(3)). The improved activities could be ascribed to a down-shift of the density of states for Mo atoms. This investigation could contribute to the design of a highly active NRR electrocatalyst.